Composites of magnetite and two-line ferrihydrite with graphite oxide (GO) were synthesized and tested as hydrogen sulfide adsorbents. Exhausted and initial composites were characterized by the adsorption of nitrogen, X-ray diffraction, potentiometric titration, thermal analysis, and FTIR. The addition of GO increased the surface area of the composites due to the formation of new micropores. The extent of the increase depended on the nature of the iron (hydr)oxide and the content of GO. The addition of GO did not considerably change the crystal structure but increased the number of acidic functional groups. While for the magnetite composites an increase in the H2S adsorption capacity after GO addition was found, the opposite effect was recorded for the ferrihydrite composites. That increase in the adsorption capacity was linked to the affinity of the composites to adsorb water in mesopores of specific sizes in which the reaction with basic surface groups takes place. Elemental sulfur and ferric and ferrous sulfates were detected on the surface of the exhausted samples. A redox reactive adsorption mechanism is proposed to govern the retention of hydrogen sulfide on the surface of the composites. The incorporation of GO enhances the chemical retention of H2S due to the incorporation of OH reactive groups and an increase in surface heterogeneity.